In order to overcome the shortcomings of traditional V-based catalysts, such as poor low-temperature activity, narrow temperature window, and toxicity. Therefore, the Mn-Fe-Nb/TiO2 catalysts were prepared using impregnation (IM), citric acid complexation (CA), co-precipitation (CP), hydrothermal synthesis (HY), and sol–gel (SG) methods to develop novel NH3 selective catalytic reduction (NH3-SCR) catalysts with excellent low-temperature activity, a wide temperature window, and environmental friendliness. Their NH3-SCR catalytic activity was evaluated, followed by a detailed analysis of their morphology, structure, specific surface area, chemical state, redox properties, acidity, and interactions using X-ray diffraction (XRD), Bruaner-Emmet-Teller (BET), Scanning Electron Microscopy (SEM), High Resolution Transmission Electron Microscopy (HR-TEM), X-ray photoelectron spectroscopy (XPS), H2 temperature-programmed reduction (H2-TPR), NH3 temperature-programmed desorption (NH3-TPD), and Fourier transform infrared spectroscopy (FTIR) techniques. The 5Mn-7Fe-4Nb/TiO2-SG catalyst, prepared via sol–gel, exhibited the highest denitrification (de-NOx) activity and the widest operating temperature window, achieving over 80% Nitric oxide (NO) conversion at 180–350 °C and a peak conversion of 97% at 250 °C. The XRD, BET, SEM, and HR-TEM characterization results showed that the catalyst prepared using the sol–gel method had the smallest particles, the highest specific surface area, and the greatest dispersion. XPS and NH3-TPD results revealed that the catalyst prepared using the sol–gel method possessed the highest surface adsorbed oxygen (Oα) content and the largest number of acidic sites. H2-TPR and FTIR analyses indicated that the catalyst prepared using the sol–gel method enhanced the reduction capacity and possessed the strongest interaction forces among support-active-promoter components. Steady-state kinetic tests confirmed that in the NH3-SCR reaction, the rate-determining step was the adsorption activation of NO on the catalyst surface. The sol–gel method reduced the activation energy for de-NOx reactions, enhancing the low-temperature activity of the catalyst.